All-in-One Electric Double Layer Supercapacitors Based on CH₃NH₃PbI₃ Perovskite Electrodes

Supercapacitors (SCs) are widely used energy storage devices in various applications that require instantaneous power supply and fast response times; however, the challenge for achieving high performance demands the continuous development and tailoring of electrode materials. Organic-inorganic halide perovskites (OIHPs) have recently received significant attention in electrochemical energy storage and conversion applications due to their unique properties including high charge carrier mobility, high mixed (electronic-ionic) conductivity, and presence of large oxygen vacancies. This study presents the fabrication and use of OIHPs based on methyl-ammonium lead iodide (CH₃NH₃PbI₃) and its Co²⁺- and Bi³⁺-substituted derivatives (CH₃NH₃Pb_1- Co I₃ and CH₃NH₃Pb_1- Bi I₃, respectively, where x = 0.1) as electrodes for SCs. SC devices were constructed symmetrically by sandwiching the synthesized electrode materials in a quasi-solid-state electrolyte between two TiO₂-coated FTO glasses. We discussed the optimization parameters (i.e., A-site doping, B-site doping, and controlling the stoichiometry of the anion and cation) to improve the electrochemical performance of the fabricated SCs. Furthermore, the effects of substitution ions (Co²⁺ and Bi³⁺) on the charge-discharge performance, energy and power density, defects, crystallinity, and microstructure were demonstrated. Electrochemical performances of the electrodes were analyzed by using CV, EIS, and GCPL techniques. The highest power density of 934.6 W/kg was obtained for Bi-substituted perovskite electrodes. Fabricated SC devices show good cyclability with 97.2, 96.3, and 86.6% retention of the initial capacitances after 50 cycles for pure, Co²⁺-substituted, and Bi³⁺-substituted perovskite electrodes, respectively.